Water-soluble diblock copolymer, poly(N-isopropylacrylamide)-block-poly(N-vinyl-2-pyrroridone) (PNIPAM(m)-b-PNVPn), was found to associate with fullerene (C-60), and thus C-60 can be solubilized in water. The 63C(60)/PNIPAM(m)-b-PNVPn micelle formed a core-shell micelle-like aggregate comprising a C-60/PNVP hydrophobic core and a thermoresponsive PNIPAM shell. The C-60-containing polymer micelle formation and its thermoresponsive behavior were characterized using light scattering and H-1 NMR techniques. The hydrodynamic radius (R-h) of the C-60-bound polymer micelle increased with increasing temperature, which was ascribed to the hydrophobic association between dehydrated PNIPAM shells above lower critical solution temperature (LCST). H-1 NMR data suggest that the motion of the PNIPAM block is restricted above LCST due to the dehydration of the PNIPAM shell in water. The generation of singlet oxygen by photosensitization by the C-60-bound polymer micelle was confirmed from photooxidation of 9,10-anthracenedipropionic acid. Furthermore, DNA was found to be cleaved by visible light irradiation in the presence of the C-60-bound polymer micelle. Therefore, there may be a hope for a pharmaceutical application of the C-60-bound polymer micelle to cancer photodynamic therapy. (C) 2011 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 49: 2761-2770, 2011